In situ cross-linking encapsulation has been demonstrated to be an efficient strategy for enhancing the humidity stability of perovskite solar cells(PSCs).In this study,a novel cross-linkable fullerene derivative,name...In situ cross-linking encapsulation has been demonstrated to be an efficient strategy for enhancing the humidity stability of perovskite solar cells(PSCs).In this study,a novel cross-linkable fullerene derivative,namely1-(p-benzoate-(p-methylvinylbenzene)-indolino[2,3][60]fullerene(FPPS),was readily synthesized from commercially available building blocks in two steps.This FPPS was employed as an interfacial modifier on perovskite surfaces in inverted planar p-i-n PSCs.Owing to the fast interfacial charge extraction and efficient trap passivation,PSCs based on the cross-linked FPPS(C-FPPS)exhibited excellent performance.The PSCs had a top-performing power conversion efficiency(PCE)of 17.82%with negligible hysteresis,compared to the control devices without C-PFFS(16.99%).Moreover,the strong water resistance of the C-FPPS interfacial layer distinctly enhances the ambient stability of PSC devices,exhibiting a t80(the time required to reach 80%of the initial PCE)of 300 h under high-humidity conditions.This significantly surpasses the control devices,whose t80 was only 130 h.These results demonstrate that cross-linkable fullerene derivatives can be promising interfacial materials for designing high-efficiency,hysteresis-free,air-stable PSCs.展开更多
Cross-linkable hole transport materials(x-HTMs)play a crucial role in solving the issue of interlayer mixing of solution-processed organic light-emitting diodes(OLEDs).However,issues such as energy level mismatch and ...Cross-linkable hole transport materials(x-HTMs)play a crucial role in solving the issue of interlayer mixing of solution-processed organic light-emitting diodes(OLEDs).However,issues such as energy level mismatch and low hole mobility hinder the application of x-HTMs in deep-blue OLEDs.In particular,thermally activated delayed fluorescent(TADF)emitters require HTMs with high triplet energies(E T)to ensure high exciton utilization efficiency.Here,two star-shaped cross-linkable HTMs 5-(9H-carbazol-9-yl)-N^(1),N^(3)-di(p-tolyl)-N^(1),N^(3)-bis(4-vinylphenyl)benzene-1,3-diamine(m-V-CzDPA)and N^(1),N^(1)-diphenyl-N^(3),N^(5)-di(p-tolyl)-N^(3),N^(5)-bis(4-vinylphenyl)benzene-1,3,5-triamine(m-V-DPADPA)were designed and synthesized.Owing to their aromatic torsion structures,m-V-CzDPA and m-V-DPADPA possessed high E Ts of 2.89 and 2.87 eV,respectively,which can effectively confine triplet excitons in the emitting layer(EML).The carrier diffusion coefficients of their x-HTMs,x-m-CzDPA and x-m-DPADPA,which were obtained via carrier diffusion imaging characterization were 0.54 and 0.44 cm^(2) s^(-1),respectively,thus indicating outstanding intrinsic hole transport capacity,with hole mobilities of 4.30×10^(-4) and 1.39×10^(-4) cm^(2) V^(-1) s^(-1),respectively.Solution-processed deep-blue TADF-OLEDs employing x-m-CzDPA as the HTM achieved a maximum current efficiency/maximum external quantum efficiency of 5.25 cd A^(-1)/18.06%,with CIE coordinates of(0.162,0.042).This is the first time that x-HTMs have served as efficient deep-blue TADF-OLEDs via a solution process,which also meets the latest BT.2020 standard(CIE_(y)≤0.046).展开更多
The solution-processed method for organic light-emitting diodes(OLEDs)offers the benefits of cost-effectiveness and enhanced material utilization.In the multilayer architecture of solution-processed OLEDs(SOLEDs),the ...The solution-processed method for organic light-emitting diodes(OLEDs)offers the benefits of cost-effectiveness and enhanced material utilization.In the multilayer architecture of solution-processed OLEDs(SOLEDs),the role of hole-transport materials(HTMs)is pivotal for cascade hole injection.However,commercial HTMs such as poly-(9,9-dioctylfluorene-alt-N-(4-sec-butylphenyl)-diphenylamine)(TFB)are hampered by incompatible energy levels and redissolution with overlayer solvent,prompting the exploration of cross-linkable HTMs(X-HTMs)for better performance.In this study,we have developed two novel small-molecule X-HTMs,N^(1),N^(1)′-((perfluoropropane-2,2-diyl)bis(4,1-phenylene))bis(N^(4),N^(4)-diphenyl-N^(1)-(4-vinylphenyl)benzene-1,4-diamine)(FTPA-V)and N,N′-((perfluoropropane-2,2-diyl)bis-(4,1-phenylene))bis(9-phenyl-N-(4-vinylphenyl)-9H-carbazol-3-amine)(FPCz-V),which incorporate thermally cross-linkable vinyl groups and electron-rich trifluoromethyl units.The X-HTMs enhance interfacial contact through superior film formation and solvent resistance,along with optimal energy levels.The application of X-HTMs significantly enhances the efficiencies and longevities of blue,green,and red SOLEDs.Specially,blue SOLED incorporating FPCz-V exhibits unprecedented lifetime(LT95)extending to over 150 h,setting a new record for blue SOLEDs.The electrochemistry stability,high bond dissociation energy,and triplet energy levels of X-HTMs can effectively minimize exciton annihilation and prolong the lifetime.These findings underscore the potential of X-HTM optimization to propel the development of stable solution-processed luminescent technologies.展开更多
How to obtain organic electro-optic materials with large electro-optic coefficients,high glass transition temperature,and good optical transparency remains a challenge in this field.To solve this problem,we introduce ...How to obtain organic electro-optic materials with large electro-optic coefficients,high glass transition temperature,and good optical transparency remains a challenge in this field.To solve this problem,we introduce groups that can undergo Huisgen cycloaddition reactions into the donor and electron bridge of chromophores with large hyperpolarizability using tetrahydroquinoline as the donor.Binary cross-linkable chromophores TLD1-2 with CF_(3)-TCF as the acceptor and chromophores TLD3-4 with 5Fph-TCF as the acceptor were synthesized.After poling and crosslinking,the T_(g)of TLD1/TLD2 and TLD3/TLD4 were raised to 152 and 174°C,respectively.The electro-optical coefficients of chromophores TLD1/TLD2 and TLD3/TLD4 were as high as 312 pm/V and 287 pm/V,respectively.The long-term alignment stability test showed that after being left at 85℃ for 500 h,the cross-linked film TLD3/TLD4 can still maintain more than 98%of the original electro-optical coefficient value,which is higher than that of TLD1/TLD2(93%).The chromophore TLD3-4 exhibited much blue-shifted maximum absorption wavelengths(~40 nm)compared to TLD1-2 which was beneficial for reducing optical loss in the device.The combination of high electro-optic coefficient,strong stability,and excellent optical transparency makes the TLD series of binary cross-linked materials very promising for practical high-performance electro-optic devices.展开更多
AIM:To investigate the response of the anterior and posterior corneal surface in femtosecond laser-assisted convex stromal lenticule addition keratoplasty(SLAK)combined with cross-linking(CXL)for treating keratoconus ...AIM:To investigate the response of the anterior and posterior corneal surface in femtosecond laser-assisted convex stromal lenticule addition keratoplasty(SLAK)combined with cross-linking(CXL)for treating keratoconus at the first 3mo of follow-up.METHODS:In this prospective observational study,20 eyes of 20 keratoconus patients who underwent SLAK combined with CXL were included.The morphological indices in keratometry and elevation data were recorded from the Sirius at baseline and 1 and 3mo postoperatively.The mean values of maximum keratometry(K_(max)),flat keratometry(K_(1)),and steep keratometry(K_(2))at the central,3-mm,5-mm,and 7-mm areas were measured from the curvature map.The changes in anterior and posterior corneal elevation under the best-fit sphere(BFS)radius at seven points horizontally of the center,3-mm,5-mm,and 7-mm area from the center at both nasal(N)and temporal(T)side were measured from elevation map.RESULTS:For the front corneal curvature,K_(1),and K_(2) at 3-mm,5-mm,and 7-mm of the anterior corneal surface increased significantly 1mo postoperatively(all P<0.05)and remained unchanged until 3mo(P>0.05).For the back corneal curvature,K_(1) and K_(2) along the 3-mm back meridian significantly decreased after month 1(P=0.002,0.077,respectively).Posterior K_(2)-readings along the 5-mm and 7-mm did not change after surgery(P>0.05).Anterior BFS decreased 1mo(P<0.001)postoperatively but remained unchanged until 3mo after SLAK(P>0.05).There was no change in posterior BFS before and after the surgery(P>0.05).Anterior elevation at N5,N3,central,and T5 points and posterior elevation at central and T7 points shifted backward 1mo postoperatively(all P<0.05)and remained stable until 3mo(P>0.05).CONCLUSION:The myopic SLAK combined with CXL is an economical alternative for stabilizing the corneal surface in severe keraoconus.“Pseudoprogression”occurs in the early phase postoperatively,but it is not an indicator of keratoconus progression.展开更多
Polymer binders possess significant potential in alleviating the volume expansion issues of silicon-based anodes,yet remain challenging due to insufficient interfacial interactions with individual components(Si,C,and ...Polymer binders possess significant potential in alleviating the volume expansion issues of silicon-based anodes,yet remain challenging due to insufficient interfacial interactions with individual components(Si,C,and Cu)of the anode.Herein,we report the synthesis of a stable three-dimensional network structure of the PAA-PEA(polyacrylic acid-polyether amines)polymer binder through intermolecular physicochemical dual cross-linking.By incorporating polar functional groups,the binder molecules not only form strong C-O-Si,N-Si,O=C-O-C,and O=C-O-Cu covalent bonds but also enhance non-covalent interactions with Si,C,and Cu,thereby improving adhesion between the binder and each interface of the anode.Furthermore,weak hydrogen bonds,acting as"sacrificial bonds",dissipate energy and disperse accumulated stress,improving the material flexibility.Due to the high mechanical stability of the framework,which combines both rigidity and flexibility and the coupling effect at the three interfaces,the movement and separation of electrode components are effectively restrained,significantly enhancing the cycling stability of silicon-graphite anodes.The PAA-PEA 2000 electrode exhibits a capacity retention of 78% after 500 cycles at a current density of 0.2 A g^(-1).This work provides insights into the mechanism of binders and guides the design of polymer binders for high-performance Si-based electrodes.展开更多
AIM:To compare simultaneous corneal collagen cross-linking(CXL)with intracorneal ring segment(ICRS)implantation versus successive ICRS followed by CXL and detect the impact of the timing of CXL after ICRS implantation...AIM:To compare simultaneous corneal collagen cross-linking(CXL)with intracorneal ring segment(ICRS)implantation versus successive ICRS followed by CXL and detect the impact of the timing of CXL after ICRS implantation in the successive method.METHODS:This is a retrospective study of the records of three groups of patients.Group 1 of 28 patients were operated on with simultaneous ICRS implantation and CXL,group 2 of 32 patients had ICRS implantation followed by CXL after 1mo,and group 3 of 38 patients had ICRS implantation followed by CXL after 3mo.The three groups had follow-up visits after 6,12,and 24mo.RESULTS:The preoperative data,age,and gender differences among 3 groups revealed no significant differences.The postoperative spherical equivalent and best-corrected visual acuity were improved significantly in all groups compared to the baseline,which were more evident in groups 1 and 2.The differences between preoperative and postoperative mean values of mean of K readings(Km)and maximum K reading(Kmax)at 6mo were 4.66 and 4.1 D in group 1,4.43 and 4.64 D in group 2,but 3.2 and 3.4 D in group 3,respectively.The spherical aberrations and the vertical coma showed significant postoperative changes in all groups,and trefoil showed nonsignificant changes.CONCLUSION:Simultaneous and sequential ICRS implantation and CXL at 1mo has similar Km and Kmax better postoperative changes than when both surgeries were done at three-month intervals.展开更多
Highly transparent,durable,and flexible liquid-repellent coatings are urgently needed in the realm of transparent materials,such as car windows,optical lenses,solar panels,and flexible screen materials.However,it has ...Highly transparent,durable,and flexible liquid-repellent coatings are urgently needed in the realm of transparent materials,such as car windows,optical lenses,solar panels,and flexible screen materials.However,it has been difficult to strike a balance between the robustness and flexibility of coatings constructed by a single cross-linked network design.To overcome the conundrum,this innovative approach effectively combines two distinct cross-linked networks with unique functions,thus overcoming the challenge.Through a tightly interwoven structure comprised of added crosslinking sites,the coating achieves improved liquid repellency(WCA>100°,OSA<10°),increased durability(withstands 2,000 cycles of cotton wear),enhanced flexibility(endures 5,000 cycles of bending with a bending radius of 1 mm),and maintains high transparency(over 98%in the range of 410 nm to 760 nm).Additionally,the coating with remarkable adhesion can be applied to multiple substrates,enabling large-scale preparation and easy cycling coating,thus expanding its potential applications.The architecture of this fluoride-free dual cross-linked network not only advances liquid-repellent surfaces but also provides valuable insights for the development of eco-friendly materials in the future.展开更多
Aging is a persistent topic of interest,with skin aging as its most visible manifestation,characterized by a reduction in intact collagen and elastic fibers in the dermis.Hyaluronic acid,a vital component of the extra...Aging is a persistent topic of interest,with skin aging as its most visible manifestation,characterized by a reduction in intact collagen and elastic fibers in the dermis.Hyaluronic acid,a vital component of the extracellular matrix present in the skin,has become a mainstream method for skin rejuvenation through injections.However,the rapid degradation of pure hyaluronic acid,combined with insufficient maintenance duration and often limited therapeutic effects,presents significant challenges for injectable treatments.Additionally,low patient compliance due to discomfort from needles penetrating the dermal layer further complicates its use.In this review,we summarize and compare existing interventions for skin aging,focusing on strategies to prolong the degradation cycle of hyaluronic acid,including variations in cross-linking modalities and injection techniques.We conclude that the injection of cross-linked modified hyaluronic acid via microneedles represents a promising approach to extend the degradation cycle,offering valuable insights for current therapeutic strategies.展开更多
In this study,a novel cost-effective methodology was developed to enhance the gas barrier properties and permselectivity of unfilled natural rubber(NR)/polybutadiene rubber(BR)composites through the construction of a ...In this study,a novel cost-effective methodology was developed to enhance the gas barrier properties and permselectivity of unfilled natural rubber(NR)/polybutadiene rubber(BR)composites through the construction of a heterogeneous structure using pre-vulcanized powder rubber to replace traditional fillers.The matrix material is composed of a blend of NR and BR,which is widely used in tire manufacturing.By incorporating pre-vulcanized trans-1,4-poly(isoprene-co-butadiene)(TBIR)rubber powder(pVTPR)with different cross-linking densities and contents,significant improvements in the gas barrier properties and CO_(2)permselectivity of the NR/BR/pVTPR composites were observed.The results indicated that compared to NR/BR/TBIR composites prepared through direct blending of NR,BR,and TBIR,the NR/BR/pVTPR composites exhibited markedly superior gas barrier properties.Increasing the cross-linking density of pVTPR resulted in progressive enhancement of the gas barrier properties of the NR/BR/pVTPR composite.For example,the addition of 20 phr pVTPR with a cross-linking density of 346 mol/m^(3)resulted in a 79%improvement in the oxygen barrier property of NR/BR/pVTPR compared to NR/BR,achieving a value of 5.47×10^(-14)cm^(3)·cm·cm^(-2)·s^(-1)·Pa^(-1).Similarly,the nitrogen barrier property improved by 76%compared to NR/BR,reaching 2.4×10^(-14)cm^(3)·cm·cm^(-2)·s^(-1)·Pa^(-1),which is 28%higher than the conventional inner liner material brominated butyl rubber(BIIR,PN2=3.32×10^(-14)cm^(3)·cm·cm^(-2)·s^(-1)·Pa^(-1)).Owing to its low cost,exceptional gas barrier properties,superior adhesion to various tire components,and co-vulcanization capabilities,the NR/BR/pVTPR composite has emerged as a promising alternative to butyl rubber in the inner liner of tires.Furthermore,by fine-tuning the cross-linking density of pVTPR,the high-gas-barrier NR/BR/pVTPR composites also demonstrated remarkable CO_(2)permselectivity,with a CO_(2)/N2 selectivity of 61.4 and a CO_(2)/O_(2)selectivity of 26.12.This innovation provides a novel strategy for CO_(2)capture and separation,with potential applications in future environmental and industrial processes.The multifunctional NR/BR/pVTPR composite,with its superior gas barrier properties and CO_(2)permselectivity,is expected to contribute to the development of safer,greener,and more cost-effective transportation solutions.展开更多
Selective hydrogenation of furfural to furfuryl alcohol is a great challenge in the hydrogenation field due to thermodynamic preference for hydrogenation of C=C over C=O.Herein,a novel Al_(2)O_(3)/C-u hybrid catalyst,...Selective hydrogenation of furfural to furfuryl alcohol is a great challenge in the hydrogenation field due to thermodynamic preference for hydrogenation of C=C over C=O.Herein,a novel Al_(2)O_(3)/C-u hybrid catalyst,composed of N-modified dendritic carbon networks supporting Al_(2)O_(3)nanoparticles,was successfully prepared via carbonizing the freeze-dried gel from spontaneous cross-linking of alginate,Al3+and urea.The obtained carbon-supported Al_(2)O_(3)hybrid catalyst has a high ratio (31%) of Al species in pentahedral-coordinated state.The introduction of urea enhances the surface N content,the ratio of pyrrolic N,and specific surface area of catalyst,leading to improved adsorption capacity of C=O and the accessibility of active sites.In the furfural hydrogenation reaction with isopropyl alcohol as hydrogen donor,Al_(2)O_(3)/C-u catalyst achieved a 90%conversion of furfural with 98.0% selectivity to furfuryl alcohol,outperforming that of commercial γ-Al_(2)O_(3).Moreover,Al_(2)O_(3)/C-u demonstrates excellent catalytic stability in the recycling tests attributed to the synergistic effect of abundant weak Lewis acid sites and the anchoring effect of the carbon network on Al_(2)O_(3)nanoparticles.This work provides an innovative and facile strategy for fabrication of carbon-supported Al_(2)O_(3)hybrid catalysts with rich AlVspecies,serving as a high selective hydrogenation catalyst through MPV reaction route.展开更多
LiMnxFe1-xPO_(4) is a promising cathode candidate due to its high security and the availability of a high 4.1 V operating voltage and high energy density.However,the poor electrochemical kinetics and structural instab...LiMnxFe1-xPO_(4) is a promising cathode candidate due to its high security and the availability of a high 4.1 V operating voltage and high energy density.However,the poor electrochemical kinetics and structural instability currently hinder its broader application.Herein,inspired by the hydrogen-bonded cross-linking and steric hindrance effect between short-chain polymer molecules(polyethylene glycol-400,PEG-400),the pomegranate-type LiMn_(0.5)Fe_(0.5)PO_(4)-0.5@C(P-LMFP@C)cathode materials with 3D ion/electron dual-conductive network structure were constructed through ball mill-assisted spray-drying method.The intermolecular effects of PEG-400 promote the spheroidization and uniform PEG coating of LMFP precursor,which prevents agglomeration during sintering.The 3D ion/electron dual-conductive network structure in P-LMFP@C accelerates the Li^(+)transport kinetics,improving the rate performance and cycling stability.As a result,the designed P-LMFP@C has remarkable electrochemical behavior,boasting excellent capacity retention(98%after 100 cycles at the 1C rate)and rate capability(91 mAh·g^(-1)at 20C).Such strategy introduces a novel window for designing high-performance olivine cathodes and offers compatibility with a range of energy storage materials for diverse applications.展开更多
Solid polymer electrolytes(SPEs)have become increasingly important in advanced lithium-ion batteries(LIBs)due to their improved safety and mechanical properties compared to organic liquid electrolytes.Cross-linked pol...Solid polymer electrolytes(SPEs)have become increasingly important in advanced lithium-ion batteries(LIBs)due to their improved safety and mechanical properties compared to organic liquid electrolytes.Cross-linked polymers have the potential to further improve the mechanical property without trading off Li-ion conductivity.In this study,focusing on a recently developed cross-linked SPE,i.e.,the one based on poly(vinylene carbonate)-poly(ethylene oxide)cross-linked network(PVCN),we used solid-state nuclear magnetic resonance(NMR)techniques to investigate the fundamental interaction between the chain segments and Li ions,as well as the lithium-ion motion.By utilizing homonuclear/heteronuclear correlation,CP(cross-polarization)kinetics,and spin-lattice relaxation experiments,etc.,we revealed the structural characteristics and their relations to lithium-ion mobilities.It is found that the network formation prevents poly(ethylene oxide)chains from crystallization,which could create sufficient space for segmental tumbling and Li-ion co nductio n.As such,the mechanical property is greatly improved with even higher Li-ion mobilities compared to the poly(vinylene carbonate)or poly(ethylene oxide)based SPE analogues.展开更多
Lithium-ion batteries(LIBs)benefit from an effective electrolyte system design in both terms of their safety and energy storage capability.Herein,a series of precursor membranes with high porosity were produced using ...Lithium-ion batteries(LIBs)benefit from an effective electrolyte system design in both terms of their safety and energy storage capability.Herein,a series of precursor membranes with high porosity were produced using electrospinning technology by mixing PVDF and triblock copolymer(PS-PEO-PS),resulting in a porous structure with good interconnections,which facilitates the absorbency of a large amount of electrolyte and further increases the ionic conductivity of gel polymer electrolytes(GPEs).It has been demonstrated that post-cross-linking of the precursor membranes increa ses the rigidity of the nanofibers,which allows the polymer film to be dimensionally sta ble up to 260℃while maintaining superior electrochemical properties.The obtained cross-linked GPEs(CGPEs)showed high ionic conductivity up to 4.53×10^(-3)S·cm^(-1).With the CGPE-25,the assembled Li/LiFeP04 half cells exhibited good rate capability and maintained a capacity of 99.4%and a coulombic efficiency of99.3%at 0.1 C.These results suggest that the combination of electrospinning technique and post-cross-linking is an effective method to construct polymer electrolytes with high thermal stability and steadily decent electrochemical performance,particularly useful for Lithium-ion battery applications that require high-temperature usage.展开更多
High-energy density lithium-ion batteries(LIBs)with layered high-nickel oxide cathodes(LiNi_(x)Co_(y)Mn_(1-x-y)O_(2),x≥0.8)show great promise in consumer electronics and vehicular applications.However,LiNi_(x)Co_(y)M...High-energy density lithium-ion batteries(LIBs)with layered high-nickel oxide cathodes(LiNi_(x)Co_(y)Mn_(1-x-y)O_(2),x≥0.8)show great promise in consumer electronics and vehicular applications.However,LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)faces challenges related to capacity decay caused by residual alkalis owing to high sensitivity to air.To address this issue,we propose a hazardous substances upcycling method that fundamentally mitigates alkali content and concurrently induces the emergence of an anti-air-sensitive layer on the cathode surface.Through the neutralization of polyacrylic acid(PAA)with residual alkalis and then coupling it with 3-aminopropyl triethoxysilane(KH550),a stable and ion-conductive cross-linked polymer layer is in situ integrated into the LiNi_(0.89)Co_(0.06)Mn_(0.05)O_(2)(NCM)cathode.Our characterization and measurements demonstrate its effectiveness.The NCM material exhibits impressive cycling performance,retaining 88.4%of its capacity after 200 cycles at 5 C and achieving an extraordinary specific capacity of 170.0 mA h g^(-1) at 10 C.Importantly,this layer on the NCM efficiently suppresses unfavorable phase transitions,severe electrolyte degradation,and CO_(2)gas evolution,while maintaining commendable resistance to air exposure.This surface modification strategy shows widespread potential for creating air-stable LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)cathodes,thereby advancing high-performance LIBs.展开更多
AIM:To observe the effects of femtosecond laserassisted excimer laser in situ keratomileusis combined with accelerated corneal cross-linking(FS-LASIK Xtra)on corneal densitometry after correcting for high myopia.METHO...AIM:To observe the effects of femtosecond laserassisted excimer laser in situ keratomileusis combined with accelerated corneal cross-linking(FS-LASIK Xtra)on corneal densitometry after correcting for high myopia.METHODS:In this prospectively study,130 patients underwent FS-LASIK or FS-LASIK Xtra for high myopia.Their right eyes were selected for inclusion in the study,of which 65 cases of 65 eyes in the FS-LASIK group,65 patients with 65 eyes in the FS-LASIK Xtra group.Patients were evaluated for corneal densitometry at 1,3,and 6mo postoperatively using Pentacam Scheimpflug imaging.RESULTS:Preoperative differences in corneal densitometry between the FS-LASIK and FS-LASIK Xtra groups in different ranges were not statistically significant(P>0.05).Layer-by-layer analysis revealed statistically significant differences in the anterior(120μm),central,and total layer corneal densitometry between the FS-LASIK and FS-LASIK Xtra groups at 1 and 3mo postoperatively(all P<0.05),the FS-LASIK Xtra group is higher than that of the FS-LASIK group.Analysis of different diameter ranges showed statistically significant differences between the FS-LASIK group and the FS-LASIK Xtra group at 1mo postoperatively in the ranges of 0–2,2–6,and 6–10 mm(both P<0.05);At 3mo postoperatively,the FS-LASIK Xtra group is higher than that of the FS-LASIK group in the ranges of 0–2 and 2–6 mm(P<0.05).At 6mo postoperatively,there were no statistically significant differences in corneal densitometry between the FS-LASIK group and the FS-LASIK Xtra group in different diameter ranges(all P>0.05).CONCLUSION:There is an increase in internal corneal densitometry during the early postoperative period after FS-LASIK Xtra for correction of high myopia.However,the densitometry values decreased to the level of conventional FS-LASIK at 6mo after surgery,with the most significant changes observed in the superficial central zone.展开更多
Gel polymer electrolytes(GPEs)effectively combine the advantages of high ionic conductivity and re-duce the risk of leakage associated with liquid.In this study,a chemically cross-linked gel polymer electrolyte was pr...Gel polymer electrolytes(GPEs)effectively combine the advantages of high ionic conductivity and re-duce the risk of leakage associated with liquid.In this study,a chemically cross-linked gel polymer electrolyte was prepared by in-situ polymerization using polymethyl methacrylate(PMMA)as a matrix and neopentyl glycol diacrylate(NPGDA)as cross-linking agent.The cross-linked structure of the GPE was preliminarily investigated,as well as the influence of the degree of cross-linking on its phys-ical properties.The GPE exhibited a superior conductivity of 1.391 mS cm^(-1) at 25℃.Herein,the Li|GPE|LiNi_(0.8) Co_(0.1) Mn_(0.1) O_(2) cell has an excellent capacity retention rate of 80.7%after 150 cycles at 0.5 C in addition to a high discharge specific capacity of 203 mAh g^(-1).The structure of the cathode ma-terial is shielded from the production of byproducts during the charging and discharging of lithium-ion batteries by the cross-linked PMMA GPE.展开更多
Polyimide(PI)is widely used in high-frequency communication technology due to its exceptional comprehensive properties.However,traditional PI has a relatively elevated dielectric constant and dielectric loss.Herein,th...Polyimide(PI)is widely used in high-frequency communication technology due to its exceptional comprehensive properties.However,traditional PI has a relatively elevated dielectric constant and dielectric loss.Herein,the different cross-linked structures were introduced in PI matrix and conducted a detailed discussion on the influence of cross-linking agent content and cross-linking structure type on the overall performance of PI films.In comparison to the dielectric constant of 2.9 of neat PI,PI with an interchain cross-linking structure containing 2 wt%1,3,5-tris(4-aminophenyl)benzene(TAPB)(interchain-PI-2)exhibited the reduced dielectric constant of 2.55 at 1 MHz.The PI films with intrachain crosslinking structure containing 2 wt%TAPB(intrachain-PI-2)exhibited the lowest dielectric constant of 2.35 and the minimum dielectric loss of0.0075 at 1 MHz.It was due to the more entanglement junctions of intrachain-PI resulting in decreased carrier transport.The thermal expansion coefficients of both interchain-PI and intrachain-PI films were effectively reduced.Moreover,in contrast to interchain-PI films,the intrachain-PI films maintained colorlessness and transparency as the cross-linking agent content increased.This work compared the effects of two different cross-linked structures on the performance of PI films and provided a feasible way to obtain low-k PI films with excellent comprehensive performance for 5G applications.展开更多
The use of CO_(2) as monomer to synthesize polymer materials is an important and potential applications topic from the viewpoint of green and sustainable chemistry.A new kind of CO_(2)-based polyurea(PUa)was synthesiz...The use of CO_(2) as monomer to synthesize polymer materials is an important and potential applications topic from the viewpoint of green and sustainable chemistry.A new kind of CO_(2)-based polyurea(PUa)was synthesized by polycondensation of CO_(2) with 4,7,10-trioxa-1,13-tridecanediamine and tris(2-aminoethyl)amine(TAEA).TAEA was used as cross-link reagent.The mechanical properties of PUa were significantly improved by inserted the crosslink agent of TAEA.The formed slight cross-linked PUa exhibited excellent mechanical properties with tensile strength of 26.8 MPa,elongation at break of 34%and Young’s modulus of 351 MPa.Moreover,it could be remolded for 3 times without obvious change in the mechanical properties,which are ascribed to the hydrogen bonding interaction among the main chains and the slight cross-linked structure.In addition,the synthesized CO_(2)-based PUa is of outstanding thermal performance with an initial decomposition temperature above 300℃,besides it is tolerance for a variety of organic solvents.展开更多
Dimethyl carbonate(DMC)is a crucial chemical raw material widely used in organic synthesis,lithiumion battery electrolytes,and various other fields.The current primary industrial process employs a conventional sodium ...Dimethyl carbonate(DMC)is a crucial chemical raw material widely used in organic synthesis,lithiumion battery electrolytes,and various other fields.The current primary industrial process employs a conventional sodium methoxide basic catalyst to produce DMC through the transesterification reaction between vinyl carbonate and methanol.However,the utilization of this catalyst presents several challenges during the process,including equipment corrosion,the generation of solid waste,susceptibility to deactivation,and complexities in separation and recovery.To address these limitations,a series of alkaline poly(ionic liquid)s,i.e.[DVBPIL][PHO],[DVCPIL][PHO],and[TBVPIL][PHO],with different crosslinking degrees and structures,were synthesized through the construction of cross-linked polymeric monomers and functionalization.These poly(ionic liquid)s exhibit cross-linked structures and controllable cationic and anionic characteristics.Research was conducted to investigate the effect of the cross-linking degree and structure on the catalytic performance of transesterification in synthesizing DMC.It was discovered that the appropriate cross-linking degree and structure of the[DVCPIL][PHO]catalyst resulted in a DMC yield of up to 80.6%.Furthermore,this catalyst material exhibited good stability,maintaining its catalytic activity after repeated use five times without significant changes.The results of this study demonstrate the potential for using alkaline poly(ionic liquid)s as a highly efficient and sustainable alternative to traditional catalysts for the transesterification synthesis of DMC.展开更多
基金the National Natural Science Foundation of China(Nos.21721001,51572231 and 51502252)the Natural Science Foundation of Fujian Province of China(No.2016J01264)。
文摘In situ cross-linking encapsulation has been demonstrated to be an efficient strategy for enhancing the humidity stability of perovskite solar cells(PSCs).In this study,a novel cross-linkable fullerene derivative,namely1-(p-benzoate-(p-methylvinylbenzene)-indolino[2,3][60]fullerene(FPPS),was readily synthesized from commercially available building blocks in two steps.This FPPS was employed as an interfacial modifier on perovskite surfaces in inverted planar p-i-n PSCs.Owing to the fast interfacial charge extraction and efficient trap passivation,PSCs based on the cross-linked FPPS(C-FPPS)exhibited excellent performance.The PSCs had a top-performing power conversion efficiency(PCE)of 17.82%with negligible hysteresis,compared to the control devices without C-PFFS(16.99%).Moreover,the strong water resistance of the C-FPPS interfacial layer distinctly enhances the ambient stability of PSC devices,exhibiting a t80(the time required to reach 80%of the initial PCE)of 300 h under high-humidity conditions.This significantly surpasses the control devices,whose t80 was only 130 h.These results demonstrate that cross-linkable fullerene derivatives can be promising interfacial materials for designing high-efficiency,hysteresis-free,air-stable PSCs.
基金supported by the National Key Research and Development Program of China(2021YFB3602702)the National Natural Science Foundation of China(52173180).
文摘Cross-linkable hole transport materials(x-HTMs)play a crucial role in solving the issue of interlayer mixing of solution-processed organic light-emitting diodes(OLEDs).However,issues such as energy level mismatch and low hole mobility hinder the application of x-HTMs in deep-blue OLEDs.In particular,thermally activated delayed fluorescent(TADF)emitters require HTMs with high triplet energies(E T)to ensure high exciton utilization efficiency.Here,two star-shaped cross-linkable HTMs 5-(9H-carbazol-9-yl)-N^(1),N^(3)-di(p-tolyl)-N^(1),N^(3)-bis(4-vinylphenyl)benzene-1,3-diamine(m-V-CzDPA)and N^(1),N^(1)-diphenyl-N^(3),N^(5)-di(p-tolyl)-N^(3),N^(5)-bis(4-vinylphenyl)benzene-1,3,5-triamine(m-V-DPADPA)were designed and synthesized.Owing to their aromatic torsion structures,m-V-CzDPA and m-V-DPADPA possessed high E Ts of 2.89 and 2.87 eV,respectively,which can effectively confine triplet excitons in the emitting layer(EML).The carrier diffusion coefficients of their x-HTMs,x-m-CzDPA and x-m-DPADPA,which were obtained via carrier diffusion imaging characterization were 0.54 and 0.44 cm^(2) s^(-1),respectively,thus indicating outstanding intrinsic hole transport capacity,with hole mobilities of 4.30×10^(-4) and 1.39×10^(-4) cm^(2) V^(-1) s^(-1),respectively.Solution-processed deep-blue TADF-OLEDs employing x-m-CzDPA as the HTM achieved a maximum current efficiency/maximum external quantum efficiency of 5.25 cd A^(-1)/18.06%,with CIE coordinates of(0.162,0.042).This is the first time that x-HTMs have served as efficient deep-blue TADF-OLEDs via a solution process,which also meets the latest BT.2020 standard(CIE_(y)≤0.046).
基金supported by the National Natural Science Foundation of China(22275003)Shenzhen Fundamental Research Program(JCYJ20200109140425347)+4 种基金the Development and Reform Commission of Shenzhen Municipality(XMHT20200106002)the Key-Area Research and Development Program of Guangdong Province(2019B010924003)Guangdong Basic and Applied Basic Research Foundation(2020B1515120030)provided by Guangdong Key Laboratory of Flexible Optoelectronic Materials and DevicesGuangdong International Science and Technology Cooperation Base of Optoelectronic Materials and Device Technology。
文摘The solution-processed method for organic light-emitting diodes(OLEDs)offers the benefits of cost-effectiveness and enhanced material utilization.In the multilayer architecture of solution-processed OLEDs(SOLEDs),the role of hole-transport materials(HTMs)is pivotal for cascade hole injection.However,commercial HTMs such as poly-(9,9-dioctylfluorene-alt-N-(4-sec-butylphenyl)-diphenylamine)(TFB)are hampered by incompatible energy levels and redissolution with overlayer solvent,prompting the exploration of cross-linkable HTMs(X-HTMs)for better performance.In this study,we have developed two novel small-molecule X-HTMs,N^(1),N^(1)′-((perfluoropropane-2,2-diyl)bis(4,1-phenylene))bis(N^(4),N^(4)-diphenyl-N^(1)-(4-vinylphenyl)benzene-1,4-diamine)(FTPA-V)and N,N′-((perfluoropropane-2,2-diyl)bis-(4,1-phenylene))bis(9-phenyl-N-(4-vinylphenyl)-9H-carbazol-3-amine)(FPCz-V),which incorporate thermally cross-linkable vinyl groups and electron-rich trifluoromethyl units.The X-HTMs enhance interfacial contact through superior film formation and solvent resistance,along with optimal energy levels.The application of X-HTMs significantly enhances the efficiencies and longevities of blue,green,and red SOLEDs.Specially,blue SOLED incorporating FPCz-V exhibits unprecedented lifetime(LT95)extending to over 150 h,setting a new record for blue SOLEDs.The electrochemistry stability,high bond dissociation energy,and triplet energy levels of X-HTMs can effectively minimize exciton annihilation and prolong the lifetime.These findings underscore the potential of X-HTM optimization to propel the development of stable solution-processed luminescent technologies.
基金supported by the Guangzhou Municipal Science and Technology Project(No.202102010426)the National Natural Science Foundation of China(Nos.21805049 and 22074025)Engineering Research Centre of Photonic Design Software,Ministry of Education,China(No.62175267).
文摘How to obtain organic electro-optic materials with large electro-optic coefficients,high glass transition temperature,and good optical transparency remains a challenge in this field.To solve this problem,we introduce groups that can undergo Huisgen cycloaddition reactions into the donor and electron bridge of chromophores with large hyperpolarizability using tetrahydroquinoline as the donor.Binary cross-linkable chromophores TLD1-2 with CF_(3)-TCF as the acceptor and chromophores TLD3-4 with 5Fph-TCF as the acceptor were synthesized.After poling and crosslinking,the T_(g)of TLD1/TLD2 and TLD3/TLD4 were raised to 152 and 174°C,respectively.The electro-optical coefficients of chromophores TLD1/TLD2 and TLD3/TLD4 were as high as 312 pm/V and 287 pm/V,respectively.The long-term alignment stability test showed that after being left at 85℃ for 500 h,the cross-linked film TLD3/TLD4 can still maintain more than 98%of the original electro-optical coefficient value,which is higher than that of TLD1/TLD2(93%).The chromophore TLD3-4 exhibited much blue-shifted maximum absorption wavelengths(~40 nm)compared to TLD1-2 which was beneficial for reducing optical loss in the device.The combination of high electro-optic coefficient,strong stability,and excellent optical transparency makes the TLD series of binary cross-linked materials very promising for practical high-performance electro-optic devices.
基金Supported by the Social Development Grant of Shaanxi Province(No.2022SF-404)the Science and Technology Program of Xi’an,China(No.23YXYJ0010,No.23YXYJ0037)+1 种基金the Research Project of Xi’an Health Commission(No.2024ms05)the Technology Innovation Supporting Program of Shaanxi(No.2024RS-CXTD-11).
文摘AIM:To investigate the response of the anterior and posterior corneal surface in femtosecond laser-assisted convex stromal lenticule addition keratoplasty(SLAK)combined with cross-linking(CXL)for treating keratoconus at the first 3mo of follow-up.METHODS:In this prospective observational study,20 eyes of 20 keratoconus patients who underwent SLAK combined with CXL were included.The morphological indices in keratometry and elevation data were recorded from the Sirius at baseline and 1 and 3mo postoperatively.The mean values of maximum keratometry(K_(max)),flat keratometry(K_(1)),and steep keratometry(K_(2))at the central,3-mm,5-mm,and 7-mm areas were measured from the curvature map.The changes in anterior and posterior corneal elevation under the best-fit sphere(BFS)radius at seven points horizontally of the center,3-mm,5-mm,and 7-mm area from the center at both nasal(N)and temporal(T)side were measured from elevation map.RESULTS:For the front corneal curvature,K_(1),and K_(2) at 3-mm,5-mm,and 7-mm of the anterior corneal surface increased significantly 1mo postoperatively(all P<0.05)and remained unchanged until 3mo(P>0.05).For the back corneal curvature,K_(1) and K_(2) along the 3-mm back meridian significantly decreased after month 1(P=0.002,0.077,respectively).Posterior K_(2)-readings along the 5-mm and 7-mm did not change after surgery(P>0.05).Anterior BFS decreased 1mo(P<0.001)postoperatively but remained unchanged until 3mo after SLAK(P>0.05).There was no change in posterior BFS before and after the surgery(P>0.05).Anterior elevation at N5,N3,central,and T5 points and posterior elevation at central and T7 points shifted backward 1mo postoperatively(all P<0.05)and remained stable until 3mo(P>0.05).CONCLUSION:The myopic SLAK combined with CXL is an economical alternative for stabilizing the corneal surface in severe keraoconus.“Pseudoprogression”occurs in the early phase postoperatively,but it is not an indicator of keratoconus progression.
基金financial support from the National Natural Science Foundation of China[grant number 21878299]。
文摘Polymer binders possess significant potential in alleviating the volume expansion issues of silicon-based anodes,yet remain challenging due to insufficient interfacial interactions with individual components(Si,C,and Cu)of the anode.Herein,we report the synthesis of a stable three-dimensional network structure of the PAA-PEA(polyacrylic acid-polyether amines)polymer binder through intermolecular physicochemical dual cross-linking.By incorporating polar functional groups,the binder molecules not only form strong C-O-Si,N-Si,O=C-O-C,and O=C-O-Cu covalent bonds but also enhance non-covalent interactions with Si,C,and Cu,thereby improving adhesion between the binder and each interface of the anode.Furthermore,weak hydrogen bonds,acting as"sacrificial bonds",dissipate energy and disperse accumulated stress,improving the material flexibility.Due to the high mechanical stability of the framework,which combines both rigidity and flexibility and the coupling effect at the three interfaces,the movement and separation of electrode components are effectively restrained,significantly enhancing the cycling stability of silicon-graphite anodes.The PAA-PEA 2000 electrode exhibits a capacity retention of 78% after 500 cycles at a current density of 0.2 A g^(-1).This work provides insights into the mechanism of binders and guides the design of polymer binders for high-performance Si-based electrodes.
文摘AIM:To compare simultaneous corneal collagen cross-linking(CXL)with intracorneal ring segment(ICRS)implantation versus successive ICRS followed by CXL and detect the impact of the timing of CXL after ICRS implantation in the successive method.METHODS:This is a retrospective study of the records of three groups of patients.Group 1 of 28 patients were operated on with simultaneous ICRS implantation and CXL,group 2 of 32 patients had ICRS implantation followed by CXL after 1mo,and group 3 of 38 patients had ICRS implantation followed by CXL after 3mo.The three groups had follow-up visits after 6,12,and 24mo.RESULTS:The preoperative data,age,and gender differences among 3 groups revealed no significant differences.The postoperative spherical equivalent and best-corrected visual acuity were improved significantly in all groups compared to the baseline,which were more evident in groups 1 and 2.The differences between preoperative and postoperative mean values of mean of K readings(Km)and maximum K reading(Kmax)at 6mo were 4.66 and 4.1 D in group 1,4.43 and 4.64 D in group 2,but 3.2 and 3.4 D in group 3,respectively.The spherical aberrations and the vertical coma showed significant postoperative changes in all groups,and trefoil showed nonsignificant changes.CONCLUSION:Simultaneous and sequential ICRS implantation and CXL at 1mo has similar Km and Kmax better postoperative changes than when both surgeries were done at three-month intervals.
基金financially supported by the National Natu-ral Science Foundation of China(Nos.22375047,22378068,and 22075046)the Natural Science Foundation of Fujian Province(No.2022J01568)+2 种基金the National Key Research and Development Program of China(Nos.2022YFB3804905 and 2022YFB3804900)China Postdoctoral Science Foundation(No.2023M743437)start-up funding from Wenzhou Institute,University of Chinese Academy of Sciences(No.WIUCASQD2019002).
文摘Highly transparent,durable,and flexible liquid-repellent coatings are urgently needed in the realm of transparent materials,such as car windows,optical lenses,solar panels,and flexible screen materials.However,it has been difficult to strike a balance between the robustness and flexibility of coatings constructed by a single cross-linked network design.To overcome the conundrum,this innovative approach effectively combines two distinct cross-linked networks with unique functions,thus overcoming the challenge.Through a tightly interwoven structure comprised of added crosslinking sites,the coating achieves improved liquid repellency(WCA>100°,OSA<10°),increased durability(withstands 2,000 cycles of cotton wear),enhanced flexibility(endures 5,000 cycles of bending with a bending radius of 1 mm),and maintains high transparency(over 98%in the range of 410 nm to 760 nm).Additionally,the coating with remarkable adhesion can be applied to multiple substrates,enabling large-scale preparation and easy cycling coating,thus expanding its potential applications.The architecture of this fluoride-free dual cross-linked network not only advances liquid-repellent surfaces but also provides valuable insights for the development of eco-friendly materials in the future.
基金financial support from several corporate sponsors.Contributions were made by the National Natural Science Foundation of China(Grant No.32071332)Shenzhen Science and Technology Innovation Project(Grant No.JCYJ20210324095802006)+2 种基金Ningbo Bureau of Science and Technology(Grant No.2023Z187)TransEasy Medical Tech.Co.,Ltd.(Grant No.2021114)Shenzhen University MedTech Innovation Fund(2023YG027).
文摘Aging is a persistent topic of interest,with skin aging as its most visible manifestation,characterized by a reduction in intact collagen and elastic fibers in the dermis.Hyaluronic acid,a vital component of the extracellular matrix present in the skin,has become a mainstream method for skin rejuvenation through injections.However,the rapid degradation of pure hyaluronic acid,combined with insufficient maintenance duration and often limited therapeutic effects,presents significant challenges for injectable treatments.Additionally,low patient compliance due to discomfort from needles penetrating the dermal layer further complicates its use.In this review,we summarize and compare existing interventions for skin aging,focusing on strategies to prolong the degradation cycle of hyaluronic acid,including variations in cross-linking modalities and injection techniques.We conclude that the injection of cross-linked modified hyaluronic acid via microneedles represents a promising approach to extend the degradation cycle,offering valuable insights for current therapeutic strategies.
基金supported by the National Key Research and Development Program of China (No. 2022YFB3704700(2022YFB3704702))the National Natural Science Foundation of China (No. 52473096)+1 种基金Major Scientific and Technological Innovation Project of Shandong Province (No. 2021CXGC010901)Taishan Scholar Program
文摘In this study,a novel cost-effective methodology was developed to enhance the gas barrier properties and permselectivity of unfilled natural rubber(NR)/polybutadiene rubber(BR)composites through the construction of a heterogeneous structure using pre-vulcanized powder rubber to replace traditional fillers.The matrix material is composed of a blend of NR and BR,which is widely used in tire manufacturing.By incorporating pre-vulcanized trans-1,4-poly(isoprene-co-butadiene)(TBIR)rubber powder(pVTPR)with different cross-linking densities and contents,significant improvements in the gas barrier properties and CO_(2)permselectivity of the NR/BR/pVTPR composites were observed.The results indicated that compared to NR/BR/TBIR composites prepared through direct blending of NR,BR,and TBIR,the NR/BR/pVTPR composites exhibited markedly superior gas barrier properties.Increasing the cross-linking density of pVTPR resulted in progressive enhancement of the gas barrier properties of the NR/BR/pVTPR composite.For example,the addition of 20 phr pVTPR with a cross-linking density of 346 mol/m^(3)resulted in a 79%improvement in the oxygen barrier property of NR/BR/pVTPR compared to NR/BR,achieving a value of 5.47×10^(-14)cm^(3)·cm·cm^(-2)·s^(-1)·Pa^(-1).Similarly,the nitrogen barrier property improved by 76%compared to NR/BR,reaching 2.4×10^(-14)cm^(3)·cm·cm^(-2)·s^(-1)·Pa^(-1),which is 28%higher than the conventional inner liner material brominated butyl rubber(BIIR,PN2=3.32×10^(-14)cm^(3)·cm·cm^(-2)·s^(-1)·Pa^(-1)).Owing to its low cost,exceptional gas barrier properties,superior adhesion to various tire components,and co-vulcanization capabilities,the NR/BR/pVTPR composite has emerged as a promising alternative to butyl rubber in the inner liner of tires.Furthermore,by fine-tuning the cross-linking density of pVTPR,the high-gas-barrier NR/BR/pVTPR composites also demonstrated remarkable CO_(2)permselectivity,with a CO_(2)/N2 selectivity of 61.4 and a CO_(2)/O_(2)selectivity of 26.12.This innovation provides a novel strategy for CO_(2)capture and separation,with potential applications in future environmental and industrial processes.The multifunctional NR/BR/pVTPR composite,with its superior gas barrier properties and CO_(2)permselectivity,is expected to contribute to the development of safer,greener,and more cost-effective transportation solutions.
基金China Postdoctoral Science Foundation (2023M733451)Dalian Innovation Team in Key Areas(2020RT06)Engineering Research Center for Key Aromatic Compounds and LiaoNing Key Laboratory,Liaoning Provincial Natural Science Foundation (Doctoral Research Start-up Fund 2024-BSBA-37)。
文摘Selective hydrogenation of furfural to furfuryl alcohol is a great challenge in the hydrogenation field due to thermodynamic preference for hydrogenation of C=C over C=O.Herein,a novel Al_(2)O_(3)/C-u hybrid catalyst,composed of N-modified dendritic carbon networks supporting Al_(2)O_(3)nanoparticles,was successfully prepared via carbonizing the freeze-dried gel from spontaneous cross-linking of alginate,Al3+and urea.The obtained carbon-supported Al_(2)O_(3)hybrid catalyst has a high ratio (31%) of Al species in pentahedral-coordinated state.The introduction of urea enhances the surface N content,the ratio of pyrrolic N,and specific surface area of catalyst,leading to improved adsorption capacity of C=O and the accessibility of active sites.In the furfural hydrogenation reaction with isopropyl alcohol as hydrogen donor,Al_(2)O_(3)/C-u catalyst achieved a 90%conversion of furfural with 98.0% selectivity to furfuryl alcohol,outperforming that of commercial γ-Al_(2)O_(3).Moreover,Al_(2)O_(3)/C-u demonstrates excellent catalytic stability in the recycling tests attributed to the synergistic effect of abundant weak Lewis acid sites and the anchoring effect of the carbon network on Al_(2)O_(3)nanoparticles.This work provides an innovative and facile strategy for fabrication of carbon-supported Al_(2)O_(3)hybrid catalysts with rich AlVspecies,serving as a high selective hydrogenation catalyst through MPV reaction route.
基金supported by the Key Technologies R&D Program of Xiamen(No.3502Z20231057)Industry Leading Key Projects of Fujian Province(No.2022H0057)+2 种基金the National Natural Science Foundation of China(No.21975212)High-Level Talent Start-Up Foundation of Xiamen Institute of Technology for financial support(No.YKJ23017R)Graduate Science and Technology Innovation Program of Xiamen University of Technology(No.YKJCX2023194).
文摘LiMnxFe1-xPO_(4) is a promising cathode candidate due to its high security and the availability of a high 4.1 V operating voltage and high energy density.However,the poor electrochemical kinetics and structural instability currently hinder its broader application.Herein,inspired by the hydrogen-bonded cross-linking and steric hindrance effect between short-chain polymer molecules(polyethylene glycol-400,PEG-400),the pomegranate-type LiMn_(0.5)Fe_(0.5)PO_(4)-0.5@C(P-LMFP@C)cathode materials with 3D ion/electron dual-conductive network structure were constructed through ball mill-assisted spray-drying method.The intermolecular effects of PEG-400 promote the spheroidization and uniform PEG coating of LMFP precursor,which prevents agglomeration during sintering.The 3D ion/electron dual-conductive network structure in P-LMFP@C accelerates the Li^(+)transport kinetics,improving the rate performance and cycling stability.As a result,the designed P-LMFP@C has remarkable electrochemical behavior,boasting excellent capacity retention(98%after 100 cycles at the 1C rate)and rate capability(91 mAh·g^(-1)at 20C).Such strategy introduces a novel window for designing high-performance olivine cathodes and offers compatibility with a range of energy storage materials for diverse applications.
基金financially supported by the National Natural Science Foundation of China(Grant No.22325405,22321002,22279153)Liaoning Revitalization Talents Program(XLYC1807207,XLYC2203134)DICP I202104。
文摘Solid polymer electrolytes(SPEs)have become increasingly important in advanced lithium-ion batteries(LIBs)due to their improved safety and mechanical properties compared to organic liquid electrolytes.Cross-linked polymers have the potential to further improve the mechanical property without trading off Li-ion conductivity.In this study,focusing on a recently developed cross-linked SPE,i.e.,the one based on poly(vinylene carbonate)-poly(ethylene oxide)cross-linked network(PVCN),we used solid-state nuclear magnetic resonance(NMR)techniques to investigate the fundamental interaction between the chain segments and Li ions,as well as the lithium-ion motion.By utilizing homonuclear/heteronuclear correlation,CP(cross-polarization)kinetics,and spin-lattice relaxation experiments,etc.,we revealed the structural characteristics and their relations to lithium-ion mobilities.It is found that the network formation prevents poly(ethylene oxide)chains from crystallization,which could create sufficient space for segmental tumbling and Li-ion co nductio n.As such,the mechanical property is greatly improved with even higher Li-ion mobilities compared to the poly(vinylene carbonate)or poly(ethylene oxide)based SPE analogues.
基金financially supported by the National Natural Science Foundation of China(Nos.21574087 and 51973128)Science and Technology Department of Sichuan Province(Nos.2019YJ0128 and 2019YFG0277)supports from the Fundamental Research Funds for the Central Universities。
文摘Lithium-ion batteries(LIBs)benefit from an effective electrolyte system design in both terms of their safety and energy storage capability.Herein,a series of precursor membranes with high porosity were produced using electrospinning technology by mixing PVDF and triblock copolymer(PS-PEO-PS),resulting in a porous structure with good interconnections,which facilitates the absorbency of a large amount of electrolyte and further increases the ionic conductivity of gel polymer electrolytes(GPEs).It has been demonstrated that post-cross-linking of the precursor membranes increa ses the rigidity of the nanofibers,which allows the polymer film to be dimensionally sta ble up to 260℃while maintaining superior electrochemical properties.The obtained cross-linked GPEs(CGPEs)showed high ionic conductivity up to 4.53×10^(-3)S·cm^(-1).With the CGPE-25,the assembled Li/LiFeP04 half cells exhibited good rate capability and maintained a capacity of 99.4%and a coulombic efficiency of99.3%at 0.1 C.These results suggest that the combination of electrospinning technique and post-cross-linking is an effective method to construct polymer electrolytes with high thermal stability and steadily decent electrochemical performance,particularly useful for Lithium-ion battery applications that require high-temperature usage.
基金supported by the National Natural Science Foundation of China(52162030)the Yunnan Major Scientific and Technological Projects(202202AG050003)+4 种基金the Key Research and Development Program of Yunnan Province(202103AA080019)the Scientific Research Foundation of Kunming University of Science and Technology(20220122)the Graduate Student Top Innovative Talent Program of Kunming University of Science and Technology(CA23107M139A)the Analysis and Testing Foundation of Kunming University of Science and Technology(2023T20220122)the Shenzhen Science and Technology Program(KCXST20221021111201003)。
文摘High-energy density lithium-ion batteries(LIBs)with layered high-nickel oxide cathodes(LiNi_(x)Co_(y)Mn_(1-x-y)O_(2),x≥0.8)show great promise in consumer electronics and vehicular applications.However,LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)faces challenges related to capacity decay caused by residual alkalis owing to high sensitivity to air.To address this issue,we propose a hazardous substances upcycling method that fundamentally mitigates alkali content and concurrently induces the emergence of an anti-air-sensitive layer on the cathode surface.Through the neutralization of polyacrylic acid(PAA)with residual alkalis and then coupling it with 3-aminopropyl triethoxysilane(KH550),a stable and ion-conductive cross-linked polymer layer is in situ integrated into the LiNi_(0.89)Co_(0.06)Mn_(0.05)O_(2)(NCM)cathode.Our characterization and measurements demonstrate its effectiveness.The NCM material exhibits impressive cycling performance,retaining 88.4%of its capacity after 200 cycles at 5 C and achieving an extraordinary specific capacity of 170.0 mA h g^(-1) at 10 C.Importantly,this layer on the NCM efficiently suppresses unfavorable phase transitions,severe electrolyte degradation,and CO_(2)gas evolution,while maintaining commendable resistance to air exposure.This surface modification strategy shows widespread potential for creating air-stable LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)cathodes,thereby advancing high-performance LIBs.
基金Supported by Shandong Province Medical Staff Science and Technology Innovation Program Project(No.SDYWZGKCJH2022021).
文摘AIM:To observe the effects of femtosecond laserassisted excimer laser in situ keratomileusis combined with accelerated corneal cross-linking(FS-LASIK Xtra)on corneal densitometry after correcting for high myopia.METHODS:In this prospectively study,130 patients underwent FS-LASIK or FS-LASIK Xtra for high myopia.Their right eyes were selected for inclusion in the study,of which 65 cases of 65 eyes in the FS-LASIK group,65 patients with 65 eyes in the FS-LASIK Xtra group.Patients were evaluated for corneal densitometry at 1,3,and 6mo postoperatively using Pentacam Scheimpflug imaging.RESULTS:Preoperative differences in corneal densitometry between the FS-LASIK and FS-LASIK Xtra groups in different ranges were not statistically significant(P>0.05).Layer-by-layer analysis revealed statistically significant differences in the anterior(120μm),central,and total layer corneal densitometry between the FS-LASIK and FS-LASIK Xtra groups at 1 and 3mo postoperatively(all P<0.05),the FS-LASIK Xtra group is higher than that of the FS-LASIK group.Analysis of different diameter ranges showed statistically significant differences between the FS-LASIK group and the FS-LASIK Xtra group at 1mo postoperatively in the ranges of 0–2,2–6,and 6–10 mm(both P<0.05);At 3mo postoperatively,the FS-LASIK Xtra group is higher than that of the FS-LASIK group in the ranges of 0–2 and 2–6 mm(P<0.05).At 6mo postoperatively,there were no statistically significant differences in corneal densitometry between the FS-LASIK group and the FS-LASIK Xtra group in different diameter ranges(all P>0.05).CONCLUSION:There is an increase in internal corneal densitometry during the early postoperative period after FS-LASIK Xtra for correction of high myopia.However,the densitometry values decreased to the level of conventional FS-LASIK at 6mo after surgery,with the most significant changes observed in the superficial central zone.
基金supported by the National Natural Science Foundation of China(No.U22A20420)the Science and Technology Plan Project of Changzhou(No.CJ20235017)In addi-tion,the authors thank Jiangsu Development&Reform Commis-sion for their support.
文摘Gel polymer electrolytes(GPEs)effectively combine the advantages of high ionic conductivity and re-duce the risk of leakage associated with liquid.In this study,a chemically cross-linked gel polymer electrolyte was prepared by in-situ polymerization using polymethyl methacrylate(PMMA)as a matrix and neopentyl glycol diacrylate(NPGDA)as cross-linking agent.The cross-linked structure of the GPE was preliminarily investigated,as well as the influence of the degree of cross-linking on its phys-ical properties.The GPE exhibited a superior conductivity of 1.391 mS cm^(-1) at 25℃.Herein,the Li|GPE|LiNi_(0.8) Co_(0.1) Mn_(0.1) O_(2) cell has an excellent capacity retention rate of 80.7%after 150 cycles at 0.5 C in addition to a high discharge specific capacity of 203 mAh g^(-1).The structure of the cathode ma-terial is shielded from the production of byproducts during the charging and discharging of lithium-ion batteries by the cross-linked PMMA GPE.
基金financially supported by the National Natural Science Foundation of China(No.52103029)。
文摘Polyimide(PI)is widely used in high-frequency communication technology due to its exceptional comprehensive properties.However,traditional PI has a relatively elevated dielectric constant and dielectric loss.Herein,the different cross-linked structures were introduced in PI matrix and conducted a detailed discussion on the influence of cross-linking agent content and cross-linking structure type on the overall performance of PI films.In comparison to the dielectric constant of 2.9 of neat PI,PI with an interchain cross-linking structure containing 2 wt%1,3,5-tris(4-aminophenyl)benzene(TAPB)(interchain-PI-2)exhibited the reduced dielectric constant of 2.55 at 1 MHz.The PI films with intrachain crosslinking structure containing 2 wt%TAPB(intrachain-PI-2)exhibited the lowest dielectric constant of 2.35 and the minimum dielectric loss of0.0075 at 1 MHz.It was due to the more entanglement junctions of intrachain-PI resulting in decreased carrier transport.The thermal expansion coefficients of both interchain-PI and intrachain-PI films were effectively reduced.Moreover,in contrast to interchain-PI films,the intrachain-PI films maintained colorlessness and transparency as the cross-linking agent content increased.This work compared the effects of two different cross-linked structures on the performance of PI films and provided a feasible way to obtain low-k PI films with excellent comprehensive performance for 5G applications.
文摘The use of CO_(2) as monomer to synthesize polymer materials is an important and potential applications topic from the viewpoint of green and sustainable chemistry.A new kind of CO_(2)-based polyurea(PUa)was synthesized by polycondensation of CO_(2) with 4,7,10-trioxa-1,13-tridecanediamine and tris(2-aminoethyl)amine(TAEA).TAEA was used as cross-link reagent.The mechanical properties of PUa were significantly improved by inserted the crosslink agent of TAEA.The formed slight cross-linked PUa exhibited excellent mechanical properties with tensile strength of 26.8 MPa,elongation at break of 34%and Young’s modulus of 351 MPa.Moreover,it could be remolded for 3 times without obvious change in the mechanical properties,which are ascribed to the hydrogen bonding interaction among the main chains and the slight cross-linked structure.In addition,the synthesized CO_(2)-based PUa is of outstanding thermal performance with an initial decomposition temperature above 300℃,besides it is tolerance for a variety of organic solvents.
基金supported by the National Key Research and Development Program of China(2022YFB4101800)National Natural Science Foundation of China(22278077,22108040)+2 种基金Key Program of Qingyuan Innovation Laboratory(00221004)Research Program of Qingyuan Innovation Laboratory(00523006)Natural Science Foundation of Fujian Province(2022J02019)。
文摘Dimethyl carbonate(DMC)is a crucial chemical raw material widely used in organic synthesis,lithiumion battery electrolytes,and various other fields.The current primary industrial process employs a conventional sodium methoxide basic catalyst to produce DMC through the transesterification reaction between vinyl carbonate and methanol.However,the utilization of this catalyst presents several challenges during the process,including equipment corrosion,the generation of solid waste,susceptibility to deactivation,and complexities in separation and recovery.To address these limitations,a series of alkaline poly(ionic liquid)s,i.e.[DVBPIL][PHO],[DVCPIL][PHO],and[TBVPIL][PHO],with different crosslinking degrees and structures,were synthesized through the construction of cross-linked polymeric monomers and functionalization.These poly(ionic liquid)s exhibit cross-linked structures and controllable cationic and anionic characteristics.Research was conducted to investigate the effect of the cross-linking degree and structure on the catalytic performance of transesterification in synthesizing DMC.It was discovered that the appropriate cross-linking degree and structure of the[DVCPIL][PHO]catalyst resulted in a DMC yield of up to 80.6%.Furthermore,this catalyst material exhibited good stability,maintaining its catalytic activity after repeated use five times without significant changes.The results of this study demonstrate the potential for using alkaline poly(ionic liquid)s as a highly efficient and sustainable alternative to traditional catalysts for the transesterification synthesis of DMC.
